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RNAA data for Bi, In and Tl in 30 E3-6 chondrites accord well with trends for heated Abee (EH4) suggesting that all EH and EL samples reflect open-system, post-accretionary heating, independent of siderophile content or recovery location.
Possible interpretations of the results of the Viking Biology Experiments suggest that greater than 1 ppm of a thermally labile oxidant, perhaps H2O2, and about 10 ppm of a thermally stable oxidant are present in the martian soil. We reexamine these results and discuss implications for future missions, the search for organics on Mars, and the possible health and engineering effects for human exploration. We conclude that further characterization of the reactivity of the martian regolith materials is warrented-although if our present understanding is correct the oxidant does not pose a hazard to humans. There are difficulties in explaining the reactivity of the Martian soil by oxidants. Most bulk phase compounds that are capable of oxidizing H2O to O2 per the Gas Exchange Experiment (GEx) are thermally labile or unstable against reduction by atmospheric CO2. Models invoking trapped O2 or peroxynitrates (NOO2(-)) require an unlikely geologic history for the Viking Lander 2 site. Most suggested oxidants, including H2O2, are expected to decompose rapidly under martian UV. Nonetheless, we conclude that the best model for the martian soil contains oxidants produced by heterogeneous chemical reactions with a photochemically produced atmospheric oxidant. The GEx results may be due to catalytic decomposition of an unstable oxidizing material by H2O. We show that interfacial reaction sites covering less than 1% of the available soil surfaces could explain the Viking Biology Experiments results.
The pathways of organic chemical synthesis, the chemical evolution on the early Earth leading to life was constrained by the development of the planet by accretion and core formation. The accretion and differentiation into the core-mantle-crust-atmosphere system strongly influenced the temperature and composition of the atmosphere, surface, and interior; but large gaps persist in our understanding of these processes. The time-span over which Earth acquired its volatiles, the composition of these volatiles, and the conditions under which outgassing of volatiles occurred to form the atmosphere, are unknown. Uncertainties in existing models for Earth accretion and early planetary development allows a wide range of possible prebiotic atmospheric compositions at the time and temperature when liquid water appeared and thermally-labile organic compounds could survive. These compositions range from strongly reducing atmospheres to mildly reducing ones.
The isotopic composition of N, Ar, Ne, and He, trapped in an uncrushed sample of the antarctic shergottite EETA 79001, was analyzed by subjecting the evacuated sample to stepped heating in the presence of 100 mtorr of oxygen. The isotopic composition of nitrogen (with the delta-N-15 value of greater than 300 percent) and the elemental ratios Ar-36/N-14 and Ar-40/N-14 were covariant along mixing lines passing through the Martian atmospheric composition. The results of this and previous analyses are consistent with a two-component nitrogen system in which about 84 ppb of trapped Martian atmospheric N is mixed in variable proportions with another, more thermally labile N component during stepped heating. The isotopic Ar-36/Ar-38 ratio of the EETA 79001 is different from that of the earth atmosphere by about 25 percent.
In an attempt to improve the thermal-oxidative stability (TOS) of PMR-type polymers, the use of 1,4-phenylenebis (phenylmaleic anhydride) PPMA, was evaluated. Two series of nadic end-capped addition curing polyimides were prepared by imidizing PPMA with either 4,4'-methylene dianiline or p-phenylenediamine. The first resulted in improved solubility and increased resin flow while the latter yielded a compression molded neat resin sample with a T(sub g) of 408 C, close to 70 C higher than PME-15. The performance of these materials in long term weight loss studies was below that of PMR-15, independent of post-cure conditions. These results can be rationalized in terms of the thermal lability of the pendant phenyl groups and the incomplete imidization of the sterically congested PPMA. The preparation of model compounds as well as future research directions are discussed.
Eight different production lots of a commercial perfluoropolyether (PFPE) based on hexafluoropropene oxide (HFPO) were applied to polished metal surfaces by spinning. One of the lots repeatedly dewetted from a clean 440C steel surface, forming droplets on the surface, whereas the other seven did not dewet. This dewetting phenomenon also repeatedly occurred on 2024 aluminum and 1018 steel, but not on copper or gold. Fourier transform infrared microspectroscopy (mu-FTIR) was used to determine thickness and uniformity of the PFPE films. The dewetting lot was found to dewet from 440C steel at a film thickness greater than 520 A. A portion of the dewetting lot was heated at 316 C for 12 days in the presence of oxygen and M-50 steel. This fluid did not dewet. Sequentially, samples of the dewetting lot were filtered either with an alumina or a silica cartridge which can remove polar impurities. Neither of the filtered samples dewetted from 440C steel. It was concluded that an unknown impurity, both thermally labile and polar, present at very low concentration and undetected by our analytical techniques (FTIR, proton NMR, or F-19 NMR), was responsible for the dewetting phenomenon.
During the past three year grant period we made excellent progress in our study of the abundances and isotopic compositions of Hg and other volatile trace elements in extraterrestrial materials. As part of my startup package I received funds to construct a state-of-the-art experimental facility to study gas-solid reaction kinetics. Much of our effort was spent developing the methodology to measure the abundance and isotopic composition of Hg at ultratrace levels in solid materials. In our first study, the abundance and isotopic composition of Hg was determined in bulk samples of the Murchison (CM) and Allende (CV) carbonaceous chondrites. We have continued our study of mercury in primitive meteorites and expanded the suite of meteorites to include other members of the CM and CV chondrite group as well as CI and CO chondrites. Samples of the CI chondrite Orgueil, the CM chondrites Murray, Nogoya, and Cold Bokkeveld, the CO chondrites Kainsaz, Omans, and Isna, and the CV chondrites Vigarano, Mokoia, and Grosnaja were tested. We have developed a thermal analysis ICP-MS technique and applied it to the study of a suite of thermally labile elements (Zn, As, Se, Cd, In, Sn, Sb, Te, Hg, Au, Tl, Pb, and Bi) in geologic materials as well.
We developed a technique to measure the thermal release profiles of a suite of labile elements (Zn, As, Se, Cd, In, Sn, Sb, Te, Pt, Hg, Au, Tl, Pb, Bi). Conclusions are reached about the behavior of each element during parent-body alteration. Additional information is contained in the original extended abstract.
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Certain elements of high lability are very responsive to thermal processes, being either highly volatile during primary nebular condensation or highly mobile by postaccretionary metamorphic or shock heating. Data for highly labile elements indicate that different thermal processes were important in the genesis of each of the chondritic groups and a discussion of each is given. Contents of highly labile elements in a given group of contemporary falls differ from those of the same group that fell in Antarctica more than 0.1 Myr ago. This difference is due either to a time-dependent change in meteorite sources or, less likely, orbital variation of the meteorite flux to Earth.
Multivariate statistical analysis techniques (linear discriminant analysis and logistic regression) can provide powerful discrimination tools which are generally unfamiliar to the planetary science community. Fall parameters were used to identify a group of 17 H chondrites (Cluster 1) that were part of a coorbital stream which intersected Earth's orbit in May, from 1855 - 1895, and can be distinguished from all other H chondrite falls. Using multivariate statistical techniques, it was demonstrated that a totally different criterion, labile trace element contents - hence thermal histories - or 13 Cluster 1 meteorites are distinguishable from those of 45 non-Cluster 1 H chondrites. Here, we focus upon the principles of multivariate statistical techniques and illustrate their application using non-meteoritic and meteoritic examples.
Fall data indicate that a significant, elongate cluster of co-orbital H chondrite falls in May between 1855 and 1895 (H Cluster 1) records encounters with two or three closely spaced and probably related meteoroid stream components, each of which was met near its perihelion. Although meteorites included in the cluster vary widely in petrographic type, shock facies, and Ne-21 exposure age, they have a distinct labile trace element signature that confirms a common thermal history and, thus, a common source region within an H chondrite parent body. Hence, meteorites selected by one criterion (fall parameters) as distinguishable from all other H chondrites, are distinguished from them by another completely different criterion (contents of labile trace elements).
Conjugated polyacetylene polymers and one condensation polyene, all containing a high degree of conjugated unsaturation, were synthesized. These polymers were characterized by chemical analysis and by thermogravimetric analysis, as well as for their film-forming capability and gas/polymer interactions. It was found that those that had a high degree of conjugated unsaturation and had resonance - stabilizing groups were very thermally stable to 200 C, e.g., poly(dicyanoacetylene), poly(ethynylferrocene) and poly(phenylacetylene); while those with labile moieties, such as poly(p-formamidophenylacetylene), among others, suffered some degradation when heated in air. When subjected to gas/polymer interaction effects, the greatest change in electrical conductance was observed when ammonia was used as the gas and poly(p-nitrophenylacetylene) was the detector. Other polymers showed similar behavior. For example, poly(ethynylcarborane), considered to be an electron acceptor also showed a change in electrical conductance when exposed to ammonia, while poly(ethynylpyridine) and poly(ethylidenepyridazine) responded to carbon monoxide. However, for "fire gases" (gases from smoldering cotton), poly(ethynylferrocene) was the most responsive. Thus, the concept of polymers with different electronegativities forming charge-transfer complexes with different gases was found to be operable.
The thermodynamic conditions for exposing metastable states are established by deenergizing a material, as in melt quenching, condensation, etc. When these conditions are met, metastable states may appear because they are kinetically preferred. The understanding of these kinetic preferences is reviewed. Formation of metastable structures by melt quenching requires high resistance to crystal nucleation to deep undercooling through the labile regime between the liquidus and configurational freezing temperature, Tg. Further, the growth of the most stable phase must be thermally activated (and therefore quench-suppressible) if the metastable state is to persist at T less than Tg. In metal systems, selective alloying is often crucial to the provision of the nucleation and/or growth resistance requisite to forming various metastable structures. These alloying effects are surveyed and interpreted.
Using the isotopic compositions derived in Huss and Lewis, 1994a, abundances of the P3, HL, and P6 noble-gas components were determined for 15 diamonds separates from primitive chondrites of 8 chondrite classes. Within a meteorite class, the relative abundances of these components correlate with the petrologic subtype of the host meteorite, indicating that metamorphism is primarily responsible for the variations. Relative abundances of P3, HL, and P6 among diamond samples can be understood in terms of thermal processing of a single mixture of diamonds like those now found in CI and CM2 chondrites. With relatively gentle heating, primitive diamonds first lose their low-temperature P3 gases and a 'labile' fraction of the HL component. Mass loss associated with release of these components produces an increase in the HL and P6 content of the remaining diamond relative to unprocessed diamond. Higher temperatures initiate destruction of the main HL carrier, while the HL content of the surviving diamonds remains essentially constant. At the same time, the P6 carrier begins to preferentially lose light noble gases. Meteorites that have experienced metamorphic temperatures greater than or = 650 C have lost essentially all of their presolar diamond through chemical reactions with surrounding minerals. The P3 abundance seems to be a function only of the maximum temperature experienced by the diamonds and thus is independent of the nature of the surrounding environment. If all classes inherited the same mixture of primitive diamonds, then P3 abundances would tie together the metamorphic scales in different meteorite classes. However, if the P3 abundance indicates a higher temperature than do other thermometers applicable to the host meteorite, then the P3 abundance may contain information about heating prior to accretion. Diamonds in the least metamorphosed EH, CV, and CO chondrites seem to carry a record of pre-accretionary thermal processing.
Element contents of Ag, Au, Bi, Cd, Co, Cs, Ga, In, Rb, Sb, Se, Te, Tl, U, and Zn were analyzed, using RNAA, in 25 Antarctic and nine non-Antarctic eucrites to determine whether these two populations differ significantly in thermal history and derive from the same or different eucrite parent body. Data for these 15 elements indicate that basaltic Antarctic and non-Antarctic eucrite populations reflect the same genetic processes and, hence, come from the same parent asteroid.
In order to investigate the relative importance of dry metamorphism and aqueous alteration in the history of chondruies, chondruies were hand-picked from the Semarkona (petrographic type 3.0), Bishunpur (3. 1), Chainpur (3.4), Dhajala (3.8) and Allegan (5) chondrites, and matrix samples were extracted from the first three ordinary chondrites. The thermoluminescence (TL) properties of all the samples were measured, and appropriate subsets of the samples were analyzed by electron-microprobe and radiochemical neutron activation and the water and H-isotopic composition determined. The TL data for chondrules from Semarkona and Bishunpur scatter widely showing no unambiguous trends, although group B1 chondrules tend to have lower sensitivities and lower peak temperatures compared with group A5 chondrules. It is argued that these data reflect the variety of processes accompanying chondrule formation. The chondrules show remarkably uniform contents of the highly labile elements, indicating mineralogical control on abundance and volatile loss from silicates and loss and recondensation of mobile chalcophiles and siderophiles in some cases. Very high D/H values (up to approx. 8000% SMOW) are observed in certain Semarkona chondrules, a confirmation of earlier work. With increasing petrographic type, mean TL sensitivities of the chondrules increase, the spread of values within an individual meteorite decreases, and peak temperatures and peak widths show trends indicating that the TL is mainly produced by feldspar and that dry, thermal metamorphism is the dominant secondary process experienced by the chondrules. The TL sensitivities of matrix samples also increase with petrographic type. Chainpur matrix samples show the same spread of peak temperatures and peak widths as Chainpur chondruies, indicating metamorphism-related changes in the feldspar are responsible for the TL of the matrix. The TL data for the Semarkona and Bishunpur matrix samples provide, at best, only weak evidence for aqueous alteration, but the matrix contains H with approximately terrestrial D/H values, even though it contains much water. Secondary processes (probably aqueous alteration) presumably lowered the D/H of the matrix and certain chondrules. While chondrule properties appear to be governed primarily by formation processes and subsequent metamorphism, the matrix of Semarkona has a more complex history involving aqueous alteration as a meteorite-wide process.